Burners for conversion of methane to olefins, aromatics, and nanoparticles

ABSTRACT

Embodiments of the present disclosure describe burner configurations used in an industrial process to convert methane to olefins, aromatics, and nanoparticles/nanomaterials. Both a vitiated coflow burner and piloted turbulent burner with inhomogeneous inlets are disclosed.

CROSS-REFERENCE TO RELATED APPLICATIONS

This application is a continuation of U.S. application Ser. No. 16/340,566, filed Apr. 9, 2019, which is a National Stage Application under 35 U.S.C. 371 of International Application No. PCT/IB2017/056264, filed Oct. 10, 2017, which claims benefit of priority from U.S. Provisional Application No. 62/406,089, filed Oct. 10, 2016, the disclosures of which are incorporated herein in their entireties.

BACKGROUND

Current methods of methane conversion typically require integration of several complex catalytic reaction technologies. Efficient conversion of methane, the dominant component of natural and shale gases, into key chemical feedstock and liquid fuels remains a significant challenge in chemistry and chemical engineering. Industrial processes for methane-derived higher hydrocarbons (e.g., olefin, aromatics) have typically been based on indirect methane conversion integrating several catalytic reaction technologies.

Light olefins (e.g., ethylene and propylene) are important basic petrochemicals used to produce plastics, fibers and other chemicals. Most light olefins are produced by steam cracking. Steam cracking involves combustion and pyrolysis processes. Traditional industrial reactor processes (e.g., Hoescht process) decouple the combustion and pyrolysis processes within two or more reactor components.

SUMMARY

In general, embodiments of the present disclosure describe reactor designs for oxy-methane combustion and pyrolysis. The reactor embodiments of the present disclosure further describe an integrated burner configuration for combining both a methane/oxygen combustion process and subsequent pyrolysis of methane to form olefins (ethylene, acetylene, etc.), aromatics (benzene, naphthalene, etc.,) and nanoparticles (carbon black, carbon nanotubes, etc.).

One embodiment of the present disclosure includes a vitiated co-flow burner. The use of catalysts is also possible with the vitiated coflow burner. Another embodiment of the present disclosure includes a piloted turbulent burner with inhomogeneous inlets. In both embodiments, seed particles or the production of nanoparticles/nanomaterials may also be utilized. If such precursors are delivered in the coflow stream, then the produced nanoparticle/nanomaterials undergo further reactions to produce functionalized nanoparticles.

Embodiments of the present disclosure further describe methods of controlling secondary reactions of a burner of combustion products using injected methane comprising providing a jet flame in coaxial flow of hot combustion products from a premised vitiated coflow of gas passing through a porous plate, providing a tube positioner to translate a central tube tip and controlling the tube positioner to vary the offset heights of the central tube in a dynamic manner based on chemical inputs to yield different secondary reactions of combustion.

Embodiments of the present disclosure describe two burner configurations adaptable for industrial processes to convert methane to olefins, aromatics, and nanoparticles/nanomaterials. The details of one or more examples are set forth in the description below. Other features, objects, and advantages will be apparent from the description and from the claims.

BRIEF DESCRIPTION OF DRAWINGS

This written disclosure describes illustrative embodiments that are non-limiting and non-exhaustive. In the drawings, which are not necessarily drawn to scale, like numerals describe substantially similar components throughout the several views. Like numerals having different letter suffixes represent different instances of substantially similar components. The drawings illustrate generally, by way of example, but not by way of limitation, various embodiments discussed in the present document.

Reference is made to illustrative embodiments that are depicted in the figures, in which:

FIG. 1 illustrates a vitiated coflow burner configuration in accordance with one or more embodiments of the present disclosure.

FIG. 2 illustrates vitiated coflow burner configuration having a monolithic catalyst in accordance with one or more embodiments of the present disclosure.

FIG. 3 illustrates a schematic of an embodiment of the present disclosure including a burner wherein the tip height of the central tube is controlled.

FIG. 4 illustrates a piloted turbulent flame burner with inhomogeneous inlets in accordance with one or more embodiments of the present disclosure.

FIG. 5 illustrates a schematic of an embodiment of the present disclosure including a piloted turbulent flame burner of FIG. 4.

DETAILED DESCRIPTION

The present disclosure relates to burner configurations used in an industrial processes to convert methane and related compounds to olefins, aromatics, and nanoparticles/nanomaterials. One embodiment of the present disclosure describes a vitiated coflow burner. Another embodiment of the present disclosure describes a piloted turbulent burner with inhomogeneous inlets.

The first burner configuration is a vitiated co-flow burner 10 as shown in FIG. 1. The burner design includes a jet flame 12 in coaxial flow of hot combustion products from a premixed flame (vitiated coflow) 14. Coflow gas (CH₄/O₂) passes through a porous plate 16 prior to combustion with gas (CH₄) from central tube 18. Porous plate 16 may be generally circular centered about tube 18. Coflow gas originates from a remote vessel (not shown) with gas pressure and gas flow rate being controlled. A generally cylindrical exit collar 20 contains the jet flame 12 and coflow flames 14 and establishes a shear boundary 22 surrounding jet flame 12.

In general terms, coflow burner 10 defines two concentric tubes with an annulus that supplies premixed methane and oxygen via porous plate 16, and a blunt-tipped central tube 18 that delivers methane. Central tube 18 can be translated vertically such that a methane jet is injected into the “hot” coflow combustion gases at various positions relative to porous plate 16. The offset-height of tube 18, and thus position of the methane injection, determines the temperature at which reactions occur, and thereby determines the yield and selectivity to various products. The methane/oxygen mixture fraction (equivalence ratio) in the premixed co-flow can vary from lean to rich conditions, in order to vary the downstream temperature field, as well as the secondary reactions of combustion products with methane injected from central tube 18.

Porous plate 16 may include a porous metal, perforated plate or various metal screens. The material used for the porous plate can be selected based on material properties (e.g., thermal conductivity, metal temperature, reactivity, machinability, etc).

Catalysts can be used in the vitiated coflow burner. FIG. 2 shows an alternative embodiment of a vitiated coflow burner having a catalytic monolith 28. In this embodiment, the coflow stream passes through ceramic monolith 28 coated by catalytic materials instead of porous plate 16. A straight-channel monolith 28 is shown in FIG. 2. The catalysts partially convert the methane/oxygen to desirable products, and thereby facilitates secondary reactions with the central methane jet. Seed particles or the production of nanoparticles/nanomaterials may also be utilized, either in the central methane jet or the coflow streams. If such precursors are delivered in the coflow stream, then the produced nanoparticle/nanomaterials undergo further reactions with the central methane jet, thereby producing functionalized nanoparticles (e.g., carbon coated TiO₂, carbon coated SiO₂, etc.).

FIG. 3 illustrates a schematic of an embodiment of the present disclosure including a burner design wherein the tip height of the central tube 18 relative to porous plate 16 is mechanically or electromechanically controlled via tip positioner 30. A variety of linkages, actuators, etc., could be utilized within tip positioner 30 to translate central tube 18 relative to porous plate 16. A controller 32 can be utilized to control tip positioner 30 to adjust the position of the central tube 18 in a dynamic manner based on chemical inputs and/or desired outputs of the burner. The controller 32 could also adjust the coflow composition, e.g., from lean to rich condition in order to vary the downstream temperature field and secondary reactions of combustion products, via a flow control system 34.

The flow control system 34 includes flow supply, control and data acquisition systems. For example, methane is fed through the inner tube 18 while air/gas is fed through the outer tube. More specifically, the method includes the step of feeding the methane from a fuel supply source through a metering valve and flow meter to the central tube 18 of the burner. As described, central tube 18 is held by a positioner 30 in the flame region of the diffusion flame.

FIG. 4 illustrates a second burner configuration including a piloted turbulent burner 40 with inhomogeneous inlets. Burner 40 defines three concentric tubes 42, 44, 46 defining gas conduits for the burner. The outermost tube 42 delivers a mixture of methane and oxygen, which is used to ignite a premixed flame. This flame supplies the heat needed for pyrolysis of methane to various desired products. The innermost tube 44 delivers methane while the intermediate tube 46 delivers oxygen. The innermost tube 44 can be translated vertically (axially within intermediate tube 46) such that a methane jet is injected into the oxygen, and various levels of premixing can be achieved before the mixture reacts in the main high temperature zone (i.e., the premixed methane/oxygen flame region). The position of the methane injection and the oxygen flow rate determine the yield and selectivity to various products. The methane/oxygen mixture fraction (equivalence ratio) in the premixed co-flow jets can vary from lean to rich conditions, in order to vary the downstream temperature field, as well as the secondary reactions of combustion products with the methane/oxygen mixture from the inner tubes. Seeding particles or the production of nanoparticles/nanomaterials may also be utilized, either in the innermost tube 44 or the outermost tube 42. If such precursors are delivered in the coflow stream, then the produced nanoparticle/nanomaterials undergo further reactions with the central methane jet, thereby producing functionalized nanoparticles (e.g., carbon coated TiO₂, carbon coated SiO₂, etc.).

FIG. 5 illustrates a schematic of an embodiment of the present disclosure including a piloted turbulent burner design wherein the axial position of the innermost supply tube 44 within intermediate tube 46 is mechanically or electromechanically controlled via tube positioner 50. A variety of linkages, actuators, etc., could be utilized within tube positioner 50 to translate the innermost tube 44 relative to intermediate tube 46. For example, a controller 32 can be utilized to control tube positioner 50 to adjust the position of the innermost tube 44 in a dynamic manner based on chemical inputs and/or desired outputs of the burner. The controller 32 could also adjust the composition of the premixed coflow (CH₄ and O₂), e.g., from lean to rich condition in order to vary the downstream temperature field and secondary reactions of combustion products, via a flow control system 34. The flow control system 34 includes flow supply, control and data acquisition systems. Controller 32 can be utilized to control the flow within innermost tube 44 via flow control system 54 and the flow within intermediate tube 46 via flow control system 56.

Other embodiments of the present disclosure are possible. Although the description above contains much specificity, these should not be construed as limiting the scope of the disclosure, but as merely providing illustrations of some of the presently preferred embodiments of this disclosure. It is also contemplated that various combinations or sub-combinations of the specific features and aspects of the embodiments may be made and still fall within the scope of this disclosure. It should be understood that various features and aspects of the disclosed embodiments can be combined with or substituted for one another in order to form various embodiments. Thus, it is intended that the scope of at least some of the present disclosure should not be limited by the particular disclosed embodiments described above.

Thus the scope of this disclosure should be determined by the appended claims and their legal equivalents. Therefore, it will be appreciated that the scope of the present disclosure fully encompasses other embodiments which may become obvious to those skilled in the art, and that the scope of the present disclosure is accordingly to be limited by nothing other than the appended claims, in which reference to an element in the singular is not intended to mean “one and only one” unless explicitly so stated, but rather “one or more.” All structural, chemical, and functional equivalents to the elements of the above-described preferred embodiment that are known to those of ordinary skill in the art are expressly incorporated herein by reference and are intended to be encompassed by the present claims. Moreover, it is not necessary for a device or method to address each and every problem sought to be solved by the present disclosure, for it to be encompassed by the present claims. Furthermore, no element, component, or method step in the present disclosure is intended to be dedicated to the public regardless of whether the element, component, or method step is explicitly recited in the claims.

The foregoing description of various preferred embodiments of the disclosure have been presented for purposes of illustration and description. It is not intended to be exhaustive or to limit the disclosure to the precise embodiments, and obviously many modifications and variations are possible in light of the above teaching. The example embodiments, as described above, were chosen and described in order to best explain the principles of the disclosure and its practical application to thereby enable others skilled in the art to best utilize the disclosure in various embodiments and with various modifications as are suited to the particular use contemplated. It is intended that the scope of the disclosure be defined by the claims appended hereto

Various examples have been described. These and other examples are within the scope of the following claims. 

What is claimed is:
 1. A burner for converting injected methane to olefins, aromatics and nanoparticles/nanomaterials, comprising: a plate through which a coflow gas passes including a porous plate or catalytic monolith, with a coflow flame established above the plate; a central tube passing through the plate and having a tip through which methane exits; two concentric tubes with an annulus that supplies premixed methane and oxygen via the porous plate or catalytic monolith; a tube positioner for varying an offset height of the tube tip relative to the plate; and a controller for adjusting the offset height of the tube tip based on material inputs or desired output yield.
 2. The burner of claim 1 further comprising an exit collar surrounding the plate, with said exit collar establishing a shear boundary of combustion products.
 3. The burner of claim 1, wherein the plate includes a catalytic monolith.
 4. The burner of claim 3, wherein the catalytic monolith is a ceramic monolith coated by catalytic materials.
 5. The burner of claim 3, wherein the catalytic monolith is a straight-channel monolith.
 6. The burner of claim 1, wherein the plate includes the porous plate.
 7. The burner of claim 6, wherein the porous plate is a perforated plate, a porous metal, or a metal screen.
 8. A method of controlling secondary reactions of a burner of combustion products using injected methane, the method comprising: passing a premixed vitiated coflow of gas through a porous plate or catalytic monolith to establish a premixed flame, wherein the porous plate or catalytic monolith is supplied with the premixed vitiated coflow of gas by an annulus of a coflow burner comprising two concentric tubes, wherein the central tube has a tip; establishing a jet flame in coaxial flow of hot combustion products from the premixed flame, said jet flame established by gas exiting from the central tube of the two concentric tubes; providing a tube positioner to translate the tip of the central tube to an offset height relative to the porous plate or catalytic monolith; and controlling the tube positioner to vary the offset height of the tip of the central tube in a dynamic manner based on chemical inputs, with the controlling step resulting in different secondary reactions of the hot combustion products from the premixed flame, with the gas exiting from the central tube.
 9. The method of claim 8, wherein the central tube is a blunt-tipped tube and the gas exiting the central tube is methane.
 10. The method of claim 8, wherein the coflow gas is a combination of methane and oxygen.
 11. The method of claim 8, wherein offset height of the central tube tip is controlled to provide both a methane/oxygen combustion process and subsequent pyrolysis of methane to form olefins, aromatics or nanoparticles.
 12. The method of claim 11, wherein the pyrolysis of methane forms nanoparticles selected from carbon black and carbon nanotubes.
 13. The method of claim 11, wherein the pyrolysis of methane forms ethylene or acetylene.
 14. The method of claim 11, wherein the pyrolysis of methane forms benzene or naphthalene.
 15. The method of claim 8, wherein the plate includes a catalytic monolith.
 16. The method of claim 15, wherein the catalytic monolith is a ceramic monolith coated by catalytic materials.
 17. The method of claim 8, wherein the plate includes the porous plate.
 18. The method of claim 17, wherein the porous plate is a perforated plate, a porous metal, or a metal screen. 